Hafnium oxide thin films with varying oxygen content were investigated with the goal of finding the optical signature of oxygen vacancies in the film structure. It was found that a reduction of oxygen content in the film leads to changes in both, structural and optical characteristics. Optical absorption spectroscopy, using nanoKelvin calorimetry, revealed an enhanced absorption in the near-ultraviolet (near-UV) and visible wavelength ranges for films with reduced oxygen content, which was attributed to mid-gap electronic states of oxygen vacancies. Absorption in the near-infrared was found to originate from structural defects other than oxygen vacancy. Luminescence generated by continuous-wave 355-nm laser excitation in e-beam films showed significant changes in the spectral profile with oxygen reduction and new band formation linked to oxygen vacancies. The luminescence from oxygen-vacancy states was found to have microsecond-scale lifetimes when compared with nanosecond-scale lifetimes of luminescence attributed to other structural film defects. Laser-damage testing using ultraviolet nanosecond and infrared femtosecond pulses showed a reduction of the damage threshold with increasing number of oxygen vacancies in hafnium oxide films.
The development of attosecond pump–probe experiments at high repetition rate requires the development of novel attosecond sources maintaining a sufficient number of photons per pulse. We use 7 fs, 800 nm pulses from a non-collinear optical parametric chirped pulse amplification laser system to generate few-pulse attosecond pulse trains (APTs) with a flux of >106 photons per shot in the extreme ultraviolet at a repetition rate of 100 kHz. The pulse trains have been fully characterised by recording frequency-resolved optical gating for complete reconstruction of attosecond bursts (FROG-CRAB) traces with a velocity map imaging spectrometer. For the pulse retrieval from the FROG-CRAB trace a new ensemble retrieval algorithm has been employed that enables the reconstruction of the shape of the APTs in the presence of carrier envelope phase fluctuations of the few-cycle laser system.
The generation of coherent light pulses in the extreme ultraviolet (XUV) spectral region with attosecond pulse durations constitutes the foundation of the field of attosecond science. Twenty years after the first demonstration of isolated attosecond pulses, they continue to be a unique tool enabling the observation and control of electron dynamics in atoms, molecules, and solids. It has long been identified that an increase in the repetition rate of attosecond light sources is necessary for many applications in atomic and molecular physics, surface science, and imaging. Although high harmonic generation (HHG) at repetition rates exceeding 100 kHz, showing a continuum in the cutoff region of the XUV spectrum, was already demonstrated in 2013, the number of photons per pulse was insufficient to perform pulse characterization via attosecond streaking, let alone to perform a pump-probe experiment. Here we report on the generation and full characterization of XUV attosecond pulses via HHG driven by near-single-cycle pulses at a repetition rate of 100 kHz. The high number of
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XUV photons per pulse on target enables attosecond electron streaking experiments through which the XUV pulses are determined to consist of a dominant single attosecond pulse. These results open the door for attosecond pump-probe spectroscopy studies at a repetition rate 1 or 2 orders of magnitude above current implementations.
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